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Synthesis of three-dimensionally interconnected sulfur-rich polymers for cathode materials of high-rate lithium-sulfur batteries.

Kim H, Lee J, Ahn H, Kim O, Park MJ - Nat Commun (2015)

Bottom Line: Porous trithiocyanuric acid crystals are synthesized for use as a soft template, where the ring-opening polymerization of elemental sulfur takes place along the thiol surfaces to create three-dimensionally interconnected sulfur-rich phases.Our lithium-sulfur cells display discharge capacity of 945 mAh g(-1) after 100 cycles at 0.2 C with high-capacity retention of 92%, as well as lifetimes of 450 cycles.Particularly, the organized amine groups in the crystals increase Li(+)-ion transfer rate, affording a rate performance of 1210, mAh g(-1) at 0.1 C and 730 mAh g(-1) at 5 C.

View Article: PubMed Central - PubMed

Affiliation: Department of Chemistry, Pohang University of Science and Technology (POSTECH), Pohang 790-784, Korea.

ABSTRACT
Elemental sulfur is one of the most attractive cathode active materials in lithium batteries because of its high theoretical specific capacity. Despite the positive aspect, lithium-sulfur batteries have suffered from severe capacity fading and limited rate capability. Here we report facile large-scale synthesis of a class of organosulfur compounds that could open a new chapter in designing cathode materials to advance lithium-sulfur battery technologies. Porous trithiocyanuric acid crystals are synthesized for use as a soft template, where the ring-opening polymerization of elemental sulfur takes place along the thiol surfaces to create three-dimensionally interconnected sulfur-rich phases. Our lithium-sulfur cells display discharge capacity of 945 mAh g(-1) after 100 cycles at 0.2 C with high-capacity retention of 92%, as well as lifetimes of 450 cycles. Particularly, the organized amine groups in the crystals increase Li(+)-ion transfer rate, affording a rate performance of 1210, mAh g(-1) at 0.1 C and 730 mAh g(-1) at 5 C.

No MeSH data available.


Related in: MedlinePlus

High-capacity and high-rate Li–S battery.(a) The discharge/charge capacities and Coulombic efficiencies of the Li/S-TTCA-I and Li/S-TTCA-II cells for 300 cycles at different C rates. (b) Representative voltammograms of the S-TTCA-I cathode obtained at different scan rates and (c) Li+-ion diffusion coefficients of the S-TTCA-I, S-TTCA-II and S–C cathodes, calculated using the Randles–Sevcik equation. (d) Rate performance of the Li/S-TTCA-I cell, compared with that of the Li/S–C cell.
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f6: High-capacity and high-rate Li–S battery.(a) The discharge/charge capacities and Coulombic efficiencies of the Li/S-TTCA-I and Li/S-TTCA-II cells for 300 cycles at different C rates. (b) Representative voltammograms of the S-TTCA-I cathode obtained at different scan rates and (c) Li+-ion diffusion coefficients of the S-TTCA-I, S-TTCA-II and S–C cathodes, calculated using the Randles–Sevcik equation. (d) Rate performance of the Li/S-TTCA-I cell, compared with that of the Li/S–C cell.

Mentions: The better battery performance with the S-TTCA-I cathode rather than with the S-TTCA-II cathode was repeatedly observed at different C rates with an extended life of 300 cycles. Discharge–charge capacities of the Li/S-TTCA-I and Li/S-TTCA-II cells at 0.2 and 0.5 C are shown in Fig. 6a. The Li/S-TTCA-I cell can deliver 872 mAh g−1 (at 0.2 C) and 886 mAh g−1 (at 0.5 C) after 300 cycles, with excellent capacity retention of over 85%. In contrast, low discharge capacities of 513 mAh g−1 (at 0.2 C) and 440 mAh g−1 (at 0.5 C) were attained with the S-TTCA-II cathode after 300 cycles. This clearly signals the morphological advantages of S-TTCA-I in enhancing the performance of the Li–S cells.


Synthesis of three-dimensionally interconnected sulfur-rich polymers for cathode materials of high-rate lithium-sulfur batteries.

Kim H, Lee J, Ahn H, Kim O, Park MJ - Nat Commun (2015)

High-capacity and high-rate Li–S battery.(a) The discharge/charge capacities and Coulombic efficiencies of the Li/S-TTCA-I and Li/S-TTCA-II cells for 300 cycles at different C rates. (b) Representative voltammograms of the S-TTCA-I cathode obtained at different scan rates and (c) Li+-ion diffusion coefficients of the S-TTCA-I, S-TTCA-II and S–C cathodes, calculated using the Randles–Sevcik equation. (d) Rate performance of the Li/S-TTCA-I cell, compared with that of the Li/S–C cell.
© Copyright Policy - open-access
Related In: Results  -  Collection

License
Show All Figures
getmorefigures.php?uid=PMC4490390&req=5

f6: High-capacity and high-rate Li–S battery.(a) The discharge/charge capacities and Coulombic efficiencies of the Li/S-TTCA-I and Li/S-TTCA-II cells for 300 cycles at different C rates. (b) Representative voltammograms of the S-TTCA-I cathode obtained at different scan rates and (c) Li+-ion diffusion coefficients of the S-TTCA-I, S-TTCA-II and S–C cathodes, calculated using the Randles–Sevcik equation. (d) Rate performance of the Li/S-TTCA-I cell, compared with that of the Li/S–C cell.
Mentions: The better battery performance with the S-TTCA-I cathode rather than with the S-TTCA-II cathode was repeatedly observed at different C rates with an extended life of 300 cycles. Discharge–charge capacities of the Li/S-TTCA-I and Li/S-TTCA-II cells at 0.2 and 0.5 C are shown in Fig. 6a. The Li/S-TTCA-I cell can deliver 872 mAh g−1 (at 0.2 C) and 886 mAh g−1 (at 0.5 C) after 300 cycles, with excellent capacity retention of over 85%. In contrast, low discharge capacities of 513 mAh g−1 (at 0.2 C) and 440 mAh g−1 (at 0.5 C) were attained with the S-TTCA-II cathode after 300 cycles. This clearly signals the morphological advantages of S-TTCA-I in enhancing the performance of the Li–S cells.

Bottom Line: Porous trithiocyanuric acid crystals are synthesized for use as a soft template, where the ring-opening polymerization of elemental sulfur takes place along the thiol surfaces to create three-dimensionally interconnected sulfur-rich phases.Our lithium-sulfur cells display discharge capacity of 945 mAh g(-1) after 100 cycles at 0.2 C with high-capacity retention of 92%, as well as lifetimes of 450 cycles.Particularly, the organized amine groups in the crystals increase Li(+)-ion transfer rate, affording a rate performance of 1210, mAh g(-1) at 0.1 C and 730 mAh g(-1) at 5 C.

View Article: PubMed Central - PubMed

Affiliation: Department of Chemistry, Pohang University of Science and Technology (POSTECH), Pohang 790-784, Korea.

ABSTRACT
Elemental sulfur is one of the most attractive cathode active materials in lithium batteries because of its high theoretical specific capacity. Despite the positive aspect, lithium-sulfur batteries have suffered from severe capacity fading and limited rate capability. Here we report facile large-scale synthesis of a class of organosulfur compounds that could open a new chapter in designing cathode materials to advance lithium-sulfur battery technologies. Porous trithiocyanuric acid crystals are synthesized for use as a soft template, where the ring-opening polymerization of elemental sulfur takes place along the thiol surfaces to create three-dimensionally interconnected sulfur-rich phases. Our lithium-sulfur cells display discharge capacity of 945 mAh g(-1) after 100 cycles at 0.2 C with high-capacity retention of 92%, as well as lifetimes of 450 cycles. Particularly, the organized amine groups in the crystals increase Li(+)-ion transfer rate, affording a rate performance of 1210, mAh g(-1) at 0.1 C and 730 mAh g(-1) at 5 C.

No MeSH data available.


Related in: MedlinePlus